Rubio Mercedes, Merchán Manuela, Pou-Amérigo Rosendo, Ortí Enrique
Departamento de Química Física, Instituto de Ciencia Molecular, Universitat de València, Dr. Moliner 50, Burjassot, 46100 Valencia, Spain.
Chemphyschem. 2003 Dec 15;4(12):1308-15. doi: 10.1002/cphc.200300790.
The low-energy region of the singlet-->singlet, singlet-->triplet, and triplet-->triplet electronic spectra of 2,2'-bithiophene are studied using multiconfigurational second-order perturbation theory (CASPT2) and extended atomic natural orbitals (ANO) basis sets. The computed vertical, adiabatic, and emission transition energies are in agreement with the available experimental data. The two lowest singlet excited states, 1(1)Bu and 2(1)Bu, are computed to be degenerate, a novel feature of the system to be borne in mind during the rationalization of its photophysics. As regards the observed high triplet quantum yield of the molecule, it is concluded that the triplet states 2(3)Ag and 2(3)Bu, separated about 0.4 eV from the two lowest singlet excited states, can be populated by intersystem crossing from nonplanar singlet states.
使用多组态二阶微扰理论(CASPT2)和扩展原子自然轨道(ANO)基组研究了2,2'-联噻吩单重态→单重态、单重态→三重态和三重态→三重态电子光谱的低能区域。计算得到的垂直、绝热和发射跃迁能量与现有的实验数据一致。计算得出两个最低的单重激发态1(1)Bu和2(1)Bu是简并的,这是该系统的一个新特征,在对其光物理进行合理化解释时需要牢记。关于观察到的该分子的高三重态量子产率,得出的结论是,与两个最低单重激发态相隔约0.4 eV的三重态2(3)Ag和2(3)Bu可通过非平面单重态的系间窜越而被填充。